Tris(2‐benzimidazolylmethyl)amine‐Directed Synthesis of Single‐Atom Nickel Catalysts for Electrochemical CO Production from CO 2
Autor: | Mani Balamurugan, Venkatesan Subramanian, Hui-Yun Jeong, Uk Sim, Venkata Surya Kumar Choutipalli, Hionsuck Baik, Janghyun Jo, Ki Tae Nam, Miyoung Kim |
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Rok vydání: | 2018 |
Předmět: |
inorganic chemicals
Inorganic chemistry Oxide chemistry.chemical_element 02 engineering and technology 010402 general chemistry 01 natural sciences Catalysis law.invention Metal chemistry.chemical_compound law Electrochemical reduction of carbon dioxide Graphene Organic Chemistry General Chemistry 021001 nanoscience & nanotechnology 0104 chemical sciences Nickel chemistry visual_art visual_art.visual_art_medium Reversible hydrogen electrode 0210 nano-technology Carbon monoxide |
Zdroj: | Chemistry – A European Journal. 24:18444-18454 |
ISSN: | 1521-3765 0947-6539 |
DOI: | 10.1002/chem.201803615 |
Popis: | The electrochemical reduction of carbon dioxide (CO2 ) to value-added products is a promising approach to reducing excess CO2 in the atmosphere. However, the development of electrocatalysts for highly selective and efficient electrochemical CO2 reduction has been challenging because protons are usually easier to reduce than CO2 in an aqueous electrolyte. Recently, single-atom catalysts (SACs) have been suggested as candidate CO2 reduction catalysts due to their unique catalytic properties. To prepare single-atom metal active sites, the stabilization of metal atoms over conductive supports such as graphene sheets to prevent metal aggregation is crucial. To address this issue, a facile method was developed to prepare single-atom nickel active sites on reduced graphene oxide (RGO) sheets for the selective production of carbon monoxide (CO) from CO2 . The tris(2-benzimidazolylmethyl)amine (NTB) ligand was introduced as a linker that can homogeneously disperse nickel atoms on the graphene oxide (GO) sheets. Because the NTB ligands form strong interactions with the GO sheets by π-π interactions and with nickel ions by ligation, they can effectively stabilize nickel ions on GO sheets by forming Ni(NTB)-GO complexes. High-temperature annealing of Ni(NTB)-GO under inert atmosphere produces nickel- and nitrogen-doped reduced graphene oxide sheets (Ni-N-RGO) with single-atom Ni-N4 active sites. Ni-N-RGO shows high CO2 reduction selectivity in the reduction of CO2 to CO with 97 % faradaic efficiency at -0.8 V vs. RHE (reversible hydrogen electrode). |
Databáze: | OpenAIRE |
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